Thermal aggregation of methylcellulose with different molecular weights was investigated in an aqueous system by static lightscattering technique to trace the transition of its molecular size and shape upon heating. Temperature-dependence of some rheological parameters was also examined to make a bridge between the macroscopic changes of methylcellulose and its molecular transition during thermal gelation. At 15 degrees C, the lowest temperature assessed, weight-average molecular weight M-w of methylcellulose used ranged from 43.6 x 10(3) to 37.7 x 10(4) g/mol, and z-average root-mean-square radius of gyration R-g ranged between 24.2 and 85.6 nm. M-w and R-g were almost temperature-independent within the range 15-60 degrees C for each methyleellulose (0.03 w/v%) but increased markedly at over 60 degrees C when the initial M-w was larger than approx. 30.0 X 10(4) g/mol. The Flory exponent for these methylcelluloses decreased markedly at over 60 degrees C to values corresponding to the behavior of a sphere configuration. Dynamic storage modulus G for methylcellulose (0.5 and 1 w/v%) increased with temperature in two separate stages. These transitions were almost independent of the initial M-w, and the second transition at a higher temperature coincided with the increase in M-w and R-g as well as in turbidity for methylcellulose with the initial M-w > approx. 30.0 x 10(4) g/mol. These results suggest that the gelation behavior of methylcellulose depends on its M-w; methylcellulose with relatively large M-w (e.g.,> approx. 30.0 x 10(4) g/mol) aggregates at higher temperatures (e.g., > 60 degrees C) to form compact or tightly packed configuration. The results also suggest that thermal aggregation of methylcellulose contributes to the formation of network structure between the molecules, consequently leading to the increase in modulus. (c) 2006 Elsevier Ltd. All rights reserved.